EPR optical detection of F centre pairs in alkali halides. - I : Pumping cycle kinetics and characteristics of the resonances

Abstract

The EPR of F centres in the ground and excited states was optically detected in the following alkali halide crystals: NaCl, KF, KCl, KBr, KI, RbBr, and RbI. A decrease of the radiative quantum efficiency of the F centre luminescence was observed when microwave transitions were induced between the spin levels. The mechanism responsible for this effect was an electronic tunnelling through the crystal field potential; the electron in the relaxed excited state of an F centre (F~*) is transferred nonradiatively to another nearby F centre in its ground state (F0), and leads to the momentary formation of an ¿ and an F' centre. Such a process is a function of the total spin of the F~*-F0 pair. The role played by the paired centres was confirmed by measurements at different F centre concentration. Moreover, at high optical excitation pumping rates, the population of the intermediate complexes (F'- ¿) is large enough to allow an estimation of the rate of the reverse process F' + ¿ '¨ F0 + F0.